4-methyl-1-pentene polymer compositions, and the laminates and adhesives using the compositions

ABSTRACT

The present invention relates to 4-methyl-1-pentene polymer compositions. Specifically, the present invention relates to adhesive compositions comprising the 4-methyl-1-pentene polymers used in bonding a 4-methyl-1-pentene polymer layer and a polar-group-containing resin layer, and laminates obtained by using such compositions. The 4-methyl-1-pentene polymer compositions as these adhesive compositions comprise a 4-methyl-1-pentene polymer (A); and a modified polyolefin resin (B) comprising a mixture of an unsaturated carboxylic acid-modified α-olefin polymer (B-1) whose α-olefin is selected from a group of propylene, butene-1 and 4-methyl-1-pentene and an unsaturated carboxylic acid-modified ethylene/α-olefin copolymer (B-2). In these compositions, an unsaturated carboxylic acid-modified 4-methyl-1-pentene polymer (A&#39;) showing a particular modification rate and a particular melt flow rate may be used in place of (A) and (B-1). These compositions have excellent adhesion to polar-group-containing resins having the OH group and the NH group, among others. The laminates obtained by laminating a 4-methyl-1-pentene polymer layer and a polar-group-containing resin layer via any of these compositions show excellent interlaminar adhesion (average peel strength) and yet heat resistance.

BACKGROUND OF THE INVENTION

The present invention relates to 4-methyl-1-pentene polymercompositions. It also relates to the 4-methyl-1-pentene polymercompositions showing excellent adhesion to a 4-methyl-1-pentene polymerlayer and a polar-group-containing resin layer and laminates using suchcompositions.

Up to the present, 4-methyl-1-pentene polymer is used in mold-releasingfilm, printed circuit mold-releasing materials, various containers, etc.because of its heat resistance, chemical resistance, mold-releasingproperties, transparency and other properties. However, in thoseapplication areas which require mechanical strength, gas barrierproperties and high-temperature mechanical strength, among otherproperties, it has been hoped that improvement will be made in4-methyl-1-pentene polymer.

One example of the attempt to give such properties to 4-methyl-1-pentenepolymer is to laminate 4-methyl-1-pentene polymer and apolar-group-containing resin such as ethylene/vinyl alcohol copolymerand polyamide. Ethylene/vinyl alcohol copolymer and polyamide, amongothers, have excellent gas barrier properties, and it is expected thatthe lamination of 4-methyl-1-pentene polymer and apolar-group-containing resin such as ethylene/vinyl alcohol copolymerand polyamide will make an improvement in the gas barrier propertiespossible. Furthermore, polyamide, particularly biaxially-orientedpolyamide, shows excellent rigidity, toughness, impact resistance andother properties, and it is expected that these properties of4-methyl-1-pentene polymer laminates will be improved by laminating suchpolyamide.

However, a two-layer lamination of a 4-methyl-1-pentene polymer layerand a polar-group-containing resin layer is not fit for practical usebecause the bonding of the two materials is not accomplished.

Attempts to bond these two materials have been made in the past. Forexample, Japanese Laid-open Patent Publication HEI 2-107438 discloses asan example a resin composition comprising an ethylene/α-olefin randomcopolymer, a tackifier and a modified polyolefin as an intermediatelayer of these laminates.

Moreover, the Japanese Laid-open Patent Publication HEI 2-107438discloses that polybutene-1 and/or 4-methyl-1-pentene polymer is blendedwith a modified polyolefin at least in one layer in order that thepolyolefin layer and the nylon layer are bonded with each other.

However, such conventional technology was not entirely satisfactory inthat the level of the adhesion achieved by it was low and the heatresistance of the structure bonded by it was also low.

SUMMARY OF THE INVENTION

For the sake of resolving the problem as described above, the object ofthe present invention is to provide adhesive compositions which firmlybonds with the polar-group-containing resin layer and has excellent heatresistance, particularly adhesive compositions showing excellentadhesion to both of the 4-methyl-1-pentene polymer layer and thepolar-group-containing resin layer, and those laminates using them whichhave excellent interlaminar adhesion.

Other and further objects, features and advantages of the presentinvention will appear more fully from the following description.

According to the present invention, the 4-methyl-1-pentene polymercomposition comprises 25 to 95 wt % of a 4-methyl-1-pentene polymer (A)and 5 to 75 wt % of a modified polyolefin resin (B) comprising a mixtureof an unsaturated carboxylic acid-modified α-olefin polymer (B-1) whoseα-olefin is selected from a group of propylene, butene-1 and4-methyl-1-pentene and an unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2).

Furthermore, the 4-methyl-1-pentene polymer composition of the presentinvention comprises 25 to 90 wt % of a 4-methyl-1-pentene polymer (A);0.1 to 20 wt % of an unsaturated carboxylic acid-modified α-olefinpolymer (B-1) whose α-olefin is selected from the group of propylene,butene-1 and 4-methyl-1-pentene; 4 to 60 wt % of an unsaturatedcarboxylic acid-modified ethylene/α-olefin copolymer (B-2); and 5 to 50wt % of a butene-1 polymer (C).

Moreover, the 4-methyl-1-pentene polymer composition of the presentinvention comprises 26 to 96 wt % of a 4-methyl-1-pentene polymer (A')at least part of which is modified with unsaturated carboxylic acid,whose rate of modification (in the weight ratio of the unsaturatedcarboxylic acid in the polymer to the polymer) may be 0.1 to 5 wt % andwhose melt flow rate may be 5 to 500 g/min as determined under theconditions of a temperature being 260° C. and a load being 5 kg inaccordance with ASTM D1238; and 4 to 74 wt % of an unsaturatedcarboxylic acid-modified ethylene/α-olefin copolymer (B-2).

In addition, the 4-methyl-1-pentene polymer composition of the presentinvention comprises 26 to 91 wt % of a 4-methyl-1-pentene polymer (A')at least part of which is modified with unsaturated carboxylic acid,whose rate of modification may be 0.1 to 5 wt % and whose melt flow ratemay be 5 to 500 g/min as determined under the conditions of atemperature being 260° C. and a load being 5 kg in accordance with ASTMD1238; 4 to 60 wt % of an unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2); and 5 to 50 wt % of a butene-1polymer (C).

The present invention provides laminates comprising onto apolar-group-containing resin layer and the aforementioned4-methyl-1-pentene polymer composition layer laminated thereto.

Furthermore, the present invention provides laminates comprising a4-methyl-1-pentene polymer layer, a polar-group-containing resin layer,and a layer of the aforementioned 4-methyl-1-pentene polymer compositionas the intermediate layer.

According to the present invention, adhesives using the aforementioned4-methyl-1-pentene polymer composition are provided.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

The 4-methyl-1-pentene polymer composition of the present invention usesa 4-methyl-1-pentene polymer (A) and (B), as a modified polyolefinresin, a mixture of an unsaturated carboxylic acid-modified α-olefinpolymer whose α-olefin is selected from a group of propylene, butene-1and 4-methyl-1-pentene and an unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer.

Given below is a detailed description of the components of the4-methyl-1-pentene polymer composition of the present invention.

(A) 4-Methyl-1-Pentene Polymer

The 4-methyl-1-pentene polymer used in the present invention is ahomopolymer of 4-methyl-1-pentene or a copolymer of 4-methyl-1-penteneand another α-olefin, such as the α-olefins having 2 to 20 carbon atomssuch as ethylene, propylene, 1-butene, 1-hexene, 1-octene, 1-decene,1-tetradecene and 1-octadecene, for example. The4-methyl-1-pentene/α-olefin copolymer used in the present invention isnormally a copolymer made up primarily of 4-methyl-1-pentene containingnot less than 85 mol %, preferably not less than 90 mol % of the4-methyl-1-pentene component. When the amount of the 4-methyl-1-pentenecomponent is within this range, the resultant composition showsexcellent heat resistance and adhesion.

The melt flow rate (MFR) of the 4-methyl-1-pentene polymer (A) used inthe present invention is preferably in a range of 1 to 400 g/10 min,more preferably 10 to 300 g/10 min, as determined under the conditionsof a temperature being 260° C. and a load being 5 kg in accordance withASTM D1238.

(B) Modified Polyolefin Resin

The modified polyolefin resin of the present invention comprises amixture of an unsaturated carboxylic acid-modified α-olefin polymer(B-1) whose α-olefin is selected from a group of propylene, butene-1 and4-methyl-1-pentene and an unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2).

(B-1) Unsaturated Carboxylic Acid-modified α-Olefin Polymer

The unsaturated carboxylic acid-modified α-olefin polymer used in thepresent invention comprises a one whose α-olefin is selected from agroup of propylene, butene-1 and 4-methyl-1-pentene. Specifically, theα-olefin polymer, the base polymer yet to be subjected to modificationtreatment, is obtained by using an α-olefin selected from amongpropylene, butene-1 and 4-methyl-1-pentene as a monomer, and the ratioof the aforesaid α-olefin component to the α-olefin polymer is not lessthan 80 wt %. If the amount of the aforementioned α-olefin is withinthis range, it may be used to be blended in any of the aforementionedthree α-olefins.

Furthermore, the aforementioned unsaturated carboxylic acid-modifiedα-olefin polymer may be a one obtained by copolymerizing any otherα-olefin having 2 to 20 carbon atoms, other than the aforementionedones, if the amount of such other α-olefin is not more than 20 wt %. Asexamples of such other α-olefins, ethylene, 1-hexene, 1-octene,1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene and1-eicosene, for example, can be cited.

Specific examples of the aforementioned α-olefin polymer includehomopolymers, such as polypropylene, polybutene andpoly(4-methyl-1-pentene), and copolymers such as propylene/ethylenecopolymer (random copolymer and block copolymer), butene/ethylenecopolymer, propylene/butene copolymer, butene/propylene copolymer andcopolymer of 4-methyl-1-pentene and another α-olefin having 2 to 20carbon atoms. Out of these, polypropylene, 4-methyl-1-pentenehomopolymer and copolymer of 4-methyl-1-pentene and another α-olefin arepreferable, and especially copolymers of 4-methyl-1-pentene homopolymeror 4-methyl-1-pentene and another α-olefin are ideal from a viewpoint ofheat resistance, adhesion and economics.

In the case of the aforementioned α-olefin polymer being a copolymer of4-methyl-1-pentene and another α-olefin, the comonomer is preferably1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene or1-eicosene, and those copolymers containing not less than 85 mol %, morepreferably not less than 90 mol %, of the 4-methyl-1-pentene componentare preferable.

Further, as the aforementioned α-olefin polymer, a polymer having thesame properties as those of the 4-methyl-1-pentene polymer used in the(A) component of the present invention may be used.

The unsaturated carboxylic acid modification of this base polymer cangenerally be accomplished by graft-reacting unsaturated carboxylic acid.Examples of the unsaturated carboxylic acid to be grafted in the presentinvention include unsaturated carboxylic acid or its derivatives, suchas unsaturated carboxylic acids such as maleic acid, fumaric acid,tetrahydrophthalic acid, itaconic acid, citraconic acid, crotonic acid,isocrotonic acid, endocis-bicyclo[2,2,1]hept-5-ene-2,3-dicarboxylicacid, acrylic acid and methacrylic acid, or their derivatives, includingthe acid anhydride, imide, amide, ester, etc. of the aforesaidunsaturated carboxylic acid.

Examples of such derivatives include maleimide, maleic anhydride,citraconic anhydride, monomethyl maleate and glycidyl maleate.

Out of these, unsaturated carboxylic acid or its acid anhydride arepreferable, and maleic acid,endocis-bicyclo[2,2,1]hept-5-ene-2,3-dicarboxylic acid and their acidanhydrides are especially preferable.

The method conventionally known to the public can be used to manufacturea modified material by graft-copolymerizing any one selected from amongsuch unsaturated carboxylic acid or derivatives thereof as the graftingmonomer with the aforementioned α-olefin polymer. For example, in thecase of using a 4-methyl-1-pentene polymer as the α-olefin polymer, suchmethods can be used as the melting modification method in which theaforementioned 4-methyl-1-pentene polymer is melted and a graftingmonomer is added for graft copolymerization and the solutionmodification method in which the aforementioned 4-methyl-1-pentenepolymer is dissolved in a solvent and a grafting monomer is added forgraft copolymerization.

To obtain the modified α-olefin polymer (B-1) by graft-copolymerizingthe aforementioned grafting monomer to the base polymer efficiently, thereaction may be carried out preferably in the presence of a radicalinitiator. In this case, grafting reaction may be normally carried outat a temperature of 60 to 350° C. The ratio of the radical initiatorused is normally in a range of 0.001 to 2 parts by weight against 100parts by weight of the base polymer.

Preferable examples of the radical initiator include organic peroxidessuch as dicumyl peroxide, di-tert-butyl peroxide,2,5-dimethyl-2,5-di(tert-butylperoxy)hexane,1,4-bis(tert-butylperoxyisopropyl)benzene and2,5-dimethyl-2,5-di(tert-butylperoxy)hexine-3.

The modified α-olefin polymer (B-1) of the present invention may bemodified at a modification rate in a range of 0.01 to 10 wt %,preferably 0.1 to 5 wt %, more preferably 1 to 5 wt % in terms of theweight of the grafting monomer. If the rate of graft modification iswithin the aforementioned range, the modified α-olefin polymer (B-1)shows satisfactory interlaminar adhesion to the polar-group-containingresin layer when used in the formation of a laminate.

The unsaturated carboxylic acid-modified α-olefin polymer (B-1) of thepresent invention may normally have intrinsic viscosity (which is anindex of its average molecular weight) of 0.1 to 10 dl/g, preferably 0.2to 5 dl/g, at 135° C. in the decalin solvent.

Furthermore, the unsaturated carboxylic acid-modified α-olefin polymer(B-1) of the present invention may normally have a melting point of notless than 100° C., preferably not less than 120° C., more preferably notless than 150° C., as determined by DSC.

In the case of (B-1) being an unsaturated carboxylic acid-modified4-methyl-1-pentene polymer in the present invention, the unsaturatedcarboxylic acid-modified 4-methyl-1-pentene polymer (A') at least partof which is modified may be used instead of using (A) and (B-1). In thiscase, as an example of the 4-methyl-1-pentene polymer, materials similarto the aforementioned (A) can be cited, but out of them, a homopolymerof 4-methyl-1-pentene or a copolymer of 4-methyl-1-pentene and anotherα-olefin are preferable.

In the case of the aforementioned 4-methyl-1-pentene polymer being acopolymer of 4-methyl-1-pentene and another α-olefin, preferableexamples of the comonomer include 1-decene, 1-dodecene, 1-tetradecene,1-hexadecene, 1-octadecene and 1-eicosene, and copolymers containing notless than 85 mol %, preferably not less than 90 mol %, of the4-methyl-1-pentene component are preferable.

Even in this case, the same unsaturated carboxylic acid or itsderivatives and modification method, among others, that are used in themodification as used for the aforementioned (B-1) can be used.

In the unsaturated carboxylic acid-modified 4-methyl-1-pentene polymer(A') of the present invention, the modification rate may be 0.1 to 5 wt%, preferably 1 to 5 wt %, against (A').

Furthermore, the melt flow rate (MFR) may be in a range of 5 to 500 g/10min, more preferably 10 to 400 g/10 min, especially preferably 10 to 300g/10 min, as determined under the conditions of a temperature being 260°C. and a load being 5 kg in accordance with ASTM D1238

(B-2) Unsaturated Carboxylic Acid-modified Ethylene/α-olefin Copolymer

The ethylene/α-olefin copolymer used in the unsaturated carboxylicacid-modified ethylene/α-olefin copolymer of the present invention is acopolymer of ethylene and an α-olefin having 3 to 20 carbon atoms. Asexamples of the α-olefin, propylene, 1-butene, 1-hexene, 1-octene,1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene and1-eicosene can be cited.

Out of these, propylene, 1-butene, 1-hexene and 1-octene are preferablefrom a viewpoint of adhesion.

The molar ratio of the ethylene and α-olefin that are copolymerized maybe preferably in a range of 45/55 to 95/5.

The same unsaturated carboxylic acid and modification method, amongothers, that are used in the modification as used for the aforementioned(B-1) can be used.

The modification rate of the unsaturated carboxylic acid-modifiedethylene α-olefin copolymer (B-2) of the present invention may be in arange of 0.01 to 10 wt %, preferably 0.1 to 5 wt %, more preferably 1 to5 wt % in terms of the weight of the grafting monomer. If the rate ofgraft modification is within the aforementioned range, the modifiedethylene/α-olefin copolymer (B-2) shows satisfactory interlaminaradhesion to the polar-group-containing resin layer when used in theformation of a laminate.

The melt flow rate (MFR) of the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) used in the present invention ispreferably in a range of 0.05 to 200 g/10 min, more preferably 0.1 to100 g/10 min, as determined under the conditions of a temperature being190° C. and a load being 2.16 kg in accordance with ASTM D1238.

Further, the unsaturated carboxylic acid-modified ethylene/α-olefincopolymer (B-2) of the present invention normally has a crystallizationdegree of not more than 30% as determined by X-rays.

The present invention uses a mixture of the aforementioned unsaturatedcarboxylic acid-modified α-olefin polymer (B-1) and the aforementionedunsaturated carboxylic acid-modified ethylene/α-olefin copolymer (B-2).The range of the preferable modification rate as such mixture is 0.01 to10 wt %, more preferably 0.1 to 5 wt %, especially preferably 1 to 5 wt%.

For the preparation of the mixture, the methods conventionally known tothe public can be used, such as dry blending and melt-kneading, forexample.

It is also possible, needless to say, to add (B-1) and (B-2) separatelyto the 4-methyl-1-pentene polymer.

(C) Butene-1 Polymer

The butene-1 polymer used in the present invention as desired is ahomopolymer of butene-1 or a copolymer of butene-1 and another α-olefinhaving 2 to 20 carbon atoms. In the case of the butene-1 polymer being acopolymer, such copolymer contains not less than 60 wt %, preferably notless than 80 wt %, more preferably not less than 90 wt %, of thebutene-1 component from a viewpoint of compatibility with the4-methyl-1-pentene copolymer.

Examples of other α-olefins used in the copolymerization includeα-olefins having not less than 2 to not more than 20 carbon atoms suchas ethylene, propylene, 1-hexene, 1-octene, 1-decene, 1-dodecene,1-tetradecene, 1-hexadecene and 1-octadecene. In the case of using suchother α-olefins, such α-olefins may be used singly or in combinationwith not less than two of them. Out of these, ethylene and propylene areused preferably.

The melt flow rate (MFR) of the butene-1 polymer as determined at atemperature of 190° C. and a load of 2.16 kg in accordance with ASTMD1238, as the index of its molecular weight, may be preferably 0.01 to100 g/10 min, especially 0.05 to 50 g/10 min, from a viewpoint ofcompatibility with other resin.

4-Methyl-1-Pentene Polymer Composition

The first composition of the present invention comprises:

[A] 25 to 95 wt %, preferably 35 to 92 wt %, more preferably 45 to 88 wt%, of a 4-methyl-1-pentene polymer (A); and

[B] 5 to 75 wt %, preferably 8 to 65 wt %, more preferably 12 to 55 wt%, of a modified polyolefin resin (B) comprising a mixture of anunsaturated carboxylic acid-modified α-olefin polymer (B-1) whoseα-olefin is selected from a group of propylene, butene-1 and4-methyl-1-pentene and an unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2).

In the present invention, the use as an adhesive resin of a4-methyl-1-pentene polymer to which a combination of a particularmodified α-olefin polymer selected from the unsaturated carboxylicacid-modified polyolefin resins and the unsaturated carboxylicacid-modified ethylene/α-olefin copolymer in a particular ratio inamount is compounded improves the adhesion between the4-methyl-1-pentene polymer and the resin containing polar groups such asthe OH group and the NH group and the heat resistance of the bondedstructure to a great extent, compared with the case of the use of eitherof the unsaturated carboxylic acid-modified polyolefin resins.

The concentration of the unsaturated carboxylic acid-modified α-olefinpolymer (B-1) in the composition is preferably 0.1 to 20 wt %, morepreferably 0.2 to 15 wt %, still more preferably 0.5 to 10 wt %. On theother hand, the concentration of the unsaturated carboxylicacid-modified ethylene/α-olefin copolymer (B-2) in the composition ispreferably 4 to 65 wt %, more preferably 7 to 60 wt %., still morepreferably 10 to 55 wt %.

The second composition of the present invention comprises:

[A] 25 to 90 wt %, preferably 35 to 80 wt %, more preferably 40 to 70 wt%, of a 4-methyl-1-pentene polymer (A);

[B1] 0.1 to 20 wt %, preferably 0.2 to 15 wt %, more preferably 0.5 to10 wt %, of an unsaturated carboxylic acid-modified α-olefin polymer(B-1) whose α-olefin is selected from a group of propylene, butene-1 and4-methyl-1-pentene;

[B2] 4 to 60 wt %, preferably 7 to 53 wt %, more preferably 10 to 45 wt%, of an unsaturated carboxylic acid-modified ethylene/α-olefincopolymer (B-2); and

[C] 5 to 50 wt %, preferably 7 to 40 wt %, more preferably 10 to 35 wt%, of a butene-1 polymer (C).

The third composition of the present invention comprises:

[A] 26 to 96 wt %, preferably 36 to 93 wt %, more preferably 46 to 89 wt%, of a 4-methyl-1-pentene polymer (A') at least part of which ismodified with unsaturated carboxylic acid, whose rate of modification is0.1 to 5 wt % and whose melt flow rate (MFR) is 5 to 500 g/10 min asdetermined under the conditions of a temperature being 260° C. and aload being 5 kg in accordance with ASTM D1238; and

[B] 4 to 74 wt %, preferably 7 to 64 wt %, more preferably 11 to 54 wt%, of an unsaturated carboxylic acid-modified ethylene/α-olefincopolymer (B-2).

In the third composition, a 4-methyl-1-pentene polymer (A') at leastpart of which is modified with unsaturated carboxylic acid is used inplace of a combination of an unmodified 4-methyl-1-pentene polymer (A)and an unsaturated carboxylic acid-modified α-olefin polymer (B-1). Theunsaturated carboxylic acid-modified 4-methyl-1-pentene polymer,containing a material corresponding to the aforementioned component(B-1) and yet the aforementioned component (A) as well, shows the sameeffect.

The fourth composition of the present invention comprises:

[A] 26 to 91 wt %, preferably 36 to 84 wt %, more preferably 41 to 80 wt%, of a 4-methyl-1-pentene polymer (A') at least part of which ismodified with unsaturated carboxylic acid, whose rate of modification is0.1 to 5 wt % and whose melt flow rate (MFR) is 5 to 500 g/10 min asdetermined under the conditions of a temperature being 260° C. and aload being 5 kg in accordance with ASTM D1238;

[B] 4 to 60 wt %, preferably 7 to 53 wt %, more preferably 10 to 45 wt%, of an unsaturated carboxylic acid-modified ethylene/α-olefincopolymer (B-2); and

[C] 5 to 50 wt %, preferably 7 to 40 wt %, more preferably 10 to 35 wt%, of a butene-1 polymer (C).

If the 4-methyl-1-pentene polymer (A) content of the first and secondcompositions or the 4-methyl-1-pentene polymer (A') content of the thirdand fourth compositions is below the aforementioned ranges, its adhesionto the 4-methyl-1-pentene polymer layer will decline, with the heatresistance of the bonded structure showing a declining trend. On theother hand, if the 4-methyl-1-pentene polymer (A) content of the firstand second compositions or the 4-methyl-1-pentene polymer (A') contentof the third and fourth compositions is beyond the aforementionedranges, its adhesion to the polar-group-containing resin layer will showa declining trend.

If the modified polyolefin resin content of the first composition iswithin the aforementioned range, its adhesion to thepolar-group-containing resin layer will become good, with the bondedstructure showing excellent heat resistance.

Further, if the unsaturated carboxylic acid-modified α-olefin polymer(B-1) content of the first and second compositions is below theaforementioned range, its adhesion to the polar-group-containing resinlayer will fall, with the heat resistance of the bonded structureshowing a declining trend. This trend is also observed in the case inwhich the modification rate of the 4-methyl-1-pentene polymer (A') ofthe third and fourth compositions is below the aforementioned range.

On the other hand, if the unsaturated carboxylic acid-modified α-olefinpolymer (B-1) content of the first and second compositions is beyond theaforementioned range, the composition will also show a trend of itsadhesion to the polar-group-containing resin layer to decline. Thistrend is also observed in the case in which the modification rate of the4-methyl-1-pentene polymer (A') of the third and fourth compositions isbeyond the aforementioned range.

Furthermore, if the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) content of the first to fourthcomposition is below the aforementioned range, its adhesion to thepolar-group-containing resin layer will show a declining trend. On theother hand, if the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) content of the first to fourthcomposition is beyond the aforementioned range, its adhesion to the4-methyl-1-pentene polymer layer and the polar-group-containing resinlayer will fall, with the heat resistance of the bonded structureshowing a declining trend.

Further, if the butene-1 polymer (C) content of the second or fourthcompositions is within the aforementioned range, delamination due toimpact at the adhesive interface will be prevented, and a decline in theheat resistance of the bonded structure will also be arrested.

It is presumed that since the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) component is dispersed in fineparticles in the compositions of the present invention, a favorableresult has been produced as to adhesion and heat resistance. Moreover,the addition of the butene-1 polymer (C) enables a better result to beobtained.

In this case, with respect to adhesion, heat resistance and the balancebetween them that in the aforementioned compositions, the (HbWb)/(HcWc)or (HaWa)/(HcWc) ratio may be in a range of 1/9 to 9/1, preferably 2/8to 8/2, wherein Hb (wt %) is the modification rate of (B-1), Wb is thecompounding ratio (in weight) of (B-1) to the compositions, Hc (wt %) isthe modification rate of (B-2), Wc is the compounding ratio (in weight)of (B-2) to the compositions, Ha (wt %) is the modification rate of(A'), and Wa is the compounding ratio (in weight) of (A') to thecompositions.

Laminates Comprising Laminates Obtained by Laminating a4-methyl-1-pentene Polymer Composition onto a Polar-group-containingResin

The laminates of the present invention may be of any structures, such as2-layer, 3-, 4-, 5- and not-less-than 5-layers, so long as they have a4-methyl-1-pentene polymer composition layer and apolar-group-containing resin layer.

Polar-group-containing Resin

The polar-group-containing resin of the present invention that is usedin the laminates is not limited in any particular way so long as it hasa polar group that contributes to gas barrier properties. However, itspreferable examples are those ones having the OH group or the NH groupin the repeating structural unit. As an example of the OH group, thehydroxyl group can be cited. Examples of the NH group include the amidegroup, amine group, urethane group and urea group.

Examples of the resin containing the hydroxyl group include polyvinylalcohol, ethylene/vinyl alcohol copolymer (EVOH), homopolymer orcopolymer of hydroxyl-group-containing 1-olefin, poly(hydroxystyrene)and poly(hydroxyalkylvinylether).

As the most appropriate example of the gas barrier resin, ethylene/vinylalcohol copolymer can be cited, and for example, a saponified copolymerobtained by saponifying a ethylene/vinyl acetate copolymer having anethylene content of 20 to 60 mol %, particularly 25 to 50 mol % in suchmanner that the saponification degree will be not less than 96 mol %,particularly not less than 99 mol %, is used. This ethylene/vinylalcohol saponified copolymer should have a molecular weight sufficientfor use for the formation of film and should generally have an MFR of0.1 to 50 g/10 min, particularly 0.5 to 20 g/10 min, as determined at190° C. and a load of 2.16 kg.

As examples of the amide-group-containing resin, polyamide (nylon) andpolyacrylamide can be cited. As an example of the amine-group-containingresin, polyacrylamine can be cited. As an example of theurethane-group-containing resin, polyurethane can be cited. As anexample of the urea-group-containing resin, polyurea can be cited. Outof these, polyamide is preferable.

Preferable specific examples of polyamide include nylon 6, nylon 66,nylon 610, nylon 11, nylon 612, nylon 12, nylon 46, nylon MXD6,polyhexamethyleneterephthalamide, polyhexamethylene(terephthalamide-isophthalamide) (copolymer), polyhexamethylene(terephthalamide-adipamide) (copolymer),polymethaphenylene-isophthalamide (meta-aramide) andpolyparaphenylene-terephthalamide (para-aramide). Particularly,aliphatic polyamides such as nylon 6, nylon 66, nylon 610, nylon 11,nylon 612 and nylon 12 are preferable.

These polyamides should also have a molecular weight sufficient for usefor the formation of film, and it is desirable that the polyamide shouldhave an intrinsic relative viscosity [η] of not less than 0.5 dl/g,preferably not less than 0.8 dl/g, especially not less than 1.0 dl/g, asdetermined at a temperature of 30° C. in concentrated sulfuric acid.

Laminates

Specific examples of the structure of the laminates include, but notlimited to, the following ones, wherein MPC is the 4-methyl-1-pentenepolymer composition of the present invention, EVOH is an ethylene/vinylalcohol copolymer, Ny is polyamide, and TPX is a 4-methyl-1-pentenepolymer:

2-layer structure: MPC/EVOH and MPC/Ny

3-layer structure: MPC/EVOH/MPC, MPC/Ny/MPC, TPX/MPC/EVOH, TPX/MPC/Nyand EVOH/MPC/Ny

4-layer structure: TPX/MPC/EVOH/MPC, TPX/MPC/Ny/MPC, MPC/EVOH/MPC/Ny andMPC/EVOH/MPC/TPX

5-layer structure: TPX/MPC/EVOH/MPC/TPX, TPX/MPC/Ny/MPC/TPX andTPX/MPC/EVOH/MPC/Ny

6-layer structure: TPX/MPC/EVOH/MPC/Ny/MPC

7-layer structure: TPX/MPC/EVOH/MPC/Ny/MPC/TPX

In the case of using a laminate of the present invention for film andsheet, the laminate may have normally a thickness of 5 to 500 μm,preferably 10 to 200 μm.

Furthermore, there is no particular limit to the thickness of the4-methyl-1-pentene polymer composition. In the case of using a laminateof the present invention for film and sheet, its thickness shouldnormally be in a range of 1 to 500 μm, especially 5 to 200 μm. In thecase of using the aforementioned laminate for bottles, its thickness maybe different from such range.

The laminates of the present invention themselves can be manufactured bythe methods known to the public such as extrusion coating, coextrusionand sandwich lamination. Needless to say, these laminates may containother materials such as paper substrates, non-woven fabrics, metalmaterials such as aluminum foil, and a heat sealant layer made ofpolyolefin resin.

Examples of the laminating methods include (a) a method in which the4-methyl-1-pentene polymer composition of the present invention isextrusion-coated onto the polar-group-containing resin layer previouslyformed, and a 4-methyl-1-pentene polymer layer is laminated onto it; (b)a method in which the 4-methyl-1-pentene polymer composition of thepresent invention is extruded as an adhesive in-between thepolar-group-containing resin layer and 4-methyl-1-pentene polymer layerwhich have been formed in advance and sandwich-laminated with them; (c)a method in which the 4-methyl-1-pentene polymer composition of thepresent invention and polar-group-containing resin which are used asintermediate layers are extrusion-coated onto the 4-methyl-1-pentenepolymer layer previously formed; (d) a method in which apolar-group-containing resin, the 4-methyl-1-pentene polymer compositionof the present invention and, as required, a 4-methyl-1-pentene polymerare coextruded by use of a multi-layer die to form a laminate; and (e) amethod in which the polar-group-containing resin layer, layer of the4-methyl-1-pentene polymer composition of the present invention and, asrequired, 4-methyl-1-pentene polymer layer, all of which have beenformed in advance are heated and compression-molded.

In this case, the 4-methyl-1-pentene polymer is a resin of a homopolymeror copolymer of the 4-methyl-1-pentene shown as the aforementioned (A)component, and the 4-methyl-1-pentene polymer composition of the presentinvention is used in bonding the 4-methyl-1-pentene polymer layer andthe polar-group-containing resin layer in the formation of the laminatesof the present invention.

In simultaneous multi-layer extrusion, the resins of the resin layersare melt-kneaded in the respective extruders for the resin layers andthen extruded into intended shapes through a multi-layer/multi-mold dieof the T-die or circular die structure, so that multi-layer films,multi-layer sheets, multi-layer tubes, multi-layer parisons, etc. may bemanufactured. It is also possible to manufacture multi-layer containersand preforms for containers by melting and mixing the resins of theresin layers in respective injection-molding machines for the resinlayers and then co-injection-molded or consecutively injection-moldedthe resins. The same multi-layer films and sheets can be formed bylamination methods such as sandwich lamination and extrusion coating.

The articles thus molded can take various forms such as films, sheets,parisons and pipes for bottles and tubes, and preforms for bottles andtubes, for example. The formation of bottles from parisons, pipes orpreforms can be easily accomplished by pinching off an extrudate in asplit mold and flowing a fluid into the inside. Furthermore, orientedblow-molded bottles, for example, can be obtained by cooling a pipe orpreform, heating it to an orientation temperature and orienting it inthe axial direction and at the same time blow-orienting it in thecircumferential direction by means of fluid pressure.

Such bottles, particularly those bottles whose 4-methyl-1-pentenepolymer layer is on the inner side, are suitable for use as bottles forvarious liquids and chemicals.

Furthermore, packaging containers, such as cups, trays and press-throughpacks (PTP), can be obtained by subjecting films and sheets to vacuummolding, pressure forming, extrusion molding, plug-assist forming, andother processing.

The laminates thus obtained show little heat shrinkage and haveexcellent mechanical properties at high temperatures. This can beverified by high-temperature tensile test.

Uses

The 4-methyl-1-pentene polymer compositions obtained by the presentinvention can be used as an adhesive. The laminates obtained by usingthose compositions, particularly the laminates of a 4-methyl-1-pentenepolymer layer/a polar-group-containing resin layer can be used formold-releasing film for industrial use, food packaging materials,release film for printed circuit boards and ACMs (advanced compositematerials) as aircraft components, for example.

Effects of the Invention

The 4-methyl-1-pentene polymer compositions of the present inventionfirmly bonds to the polar-group-containing resin layer and yet showsexcellent heat resistance. Especially, these compositions exhibitexcellent adhesion to both the 4-methyl-1-pentene polymer layer and thepolar-group-containing resin layer. and the resultant laminates showexcellent interlaminar adhesion. Because of this property, the4-methyl-1-pentene polymer compositions of the present invention areused as an adhesive.

EXAMPLES

In the following examples are described several preferred embodiments toillustrate the present invention. However, it is to be understood thatthe present invention is not intended to be limited to the specificembodiments.

The resin compositions used in the following Examples are as shown inTable 1 below.

                                      TABLE 1                                     __________________________________________________________________________                                          MFR                                         Modification  Measurement                                                     rate MFR Temp. [η]                                                      Type of Polymer Comonomer (wt %) (g/10 min) (° C.) (dl/g)            __________________________________________________________________________    (A)  Poly-4-methyl-                                                                         Mixture of 1-                                                                            --     20    260     --                                 pentene-1 hexadecene and 1-                                                    octadecene is 6.5                                                             wt %.                                                                       (B-1a) Maleic anhydride- 1-Decene is 3.2 wt %. 4.0 --  -- 0.4                  modified poly-4-                                                              methyl-pentene-1                                                             (B-1b) Maleic anhydride-  3.0 -- -- 0.4                                        modified PP                                                                  (B-2) Maleic anhydride- 1-Butene is 20 mol %. 1.0 0.5 230 --                   modified                                                                      ethylene/butene-1                                                             copolymer                                                                    (C) Polybutene Ethylene is 9 mol %. -- 0.2 190 --                              Nylon 6  -- --  -- 1.0                                                        EVOH  -- 5.5 190 --                                                        __________________________________________________________________________

The conditions for measuring the physical properties of the resins usedhere are as follows:

(1) Modification rate:

The carbonyl absorption band of the maleic acid of the modified materialin the infrared absorption spectrum was at 1850 cm⁻¹ and 1785 cm⁻¹ asdetermined by use of an infrared spectrophotometer (available from NihonBunko Model A-302). From this, the modification rate was determined fromthe absorbance per unit film thickness, by using a calibration curvepreviously prepared.

(2) Melt flow rate (MFR):

MFR was measured at the temperature shown in Table 1 and the load of2.16 kg [however, 5 kg for (A)] in accordance with ASTM D1238.

(3) Intrinsic viscosity ([η]):

(i) Modified polymer:

The intrinsic viscosity was measured at a temperature of 135° C. in thedecalin solvent.

(ii) Polyamide:

The intrinsic viscosity was measured in concentrated sulfuric acid at atemperature of 30° C. in accordance with the ordinary method.

Further, the compositions were prepared under the following melting andblending conditions:

Melting and blending conditions:

Extruder: Twin-screw extruder (screw diamter: 45 mm) available fromIkegai Tekko.

Extrusion temp.: Temperatures at the cylinder zones, adapter (AD) anddie (D) are as follows:

C1/C2/C3/C4/C5/C6/AD/D=240/260/260/260/260/260/260/260(° C.)

Extrusion rate: Screw rotary speed=200 rpm

Screw feed rotary speed=40 rpm

Moreover, the formation of extruded multi-layer cast film was carriedout under the following conditions:

Conditions for the formation of extruded multi-layer cast film:

Structure of a laiminate: 4-methyl-1-pentene polymer/adhesiveresin/nylon 6=40 μm/15 μm/15 μm

Resin used:

4-methyl-1-pentene polymer: 4-methyl-1-pentene/1-decene copolymer[1-decene content: 6.5 wt %; MFR(temp.: 260° C.; load: 5 kg): 20 g/10min, produced by Mitsui Chemicals]

Adhesive resin: A compound obtained by blending the components as shownin Table 1 at the compounding ratios shown in Table 2.

Nylon 6: CM1021FX (manufactured by Toray)

Extruder:

Extruder for 4-methyl-1-pentene polymer layer: Available from ModernMachinery (40 mm in diameter)

Extruder for adhesive resin: Available from Modern Machinery (40 mm indiameter)

Extruder for nylon 6 resin layer: Available from Modern Machinery (40 mmin diameter)

Processing temperature conditions: (Temperatures at the zones are shownfrom the direction of the resin inlet.)

Extruder for 4-methyl-1-pentene polymer layer:

C1/C2/C3/H(head)=270/280/280/280 (° C.)

Extruder for adhesive resin:

C1/C2/C3=200/230/230 (° C.)

Extruder for nylon 6 resin layer:

C1/C2/C3=240/260/260 (° C.)

Joint and adapter:

J/A1/A2/A3/A4=260/260/270/270/270 (° C.)

Die: D1/D2/D3=270/270/270 (° C.)

Processing speed: 7 m/min

The physical properties of the laminates obtained as described abovewere measured by the following method:

(1) Elmendorf tear strength:

Test equipment: Elmendorf tear tester (available from Toyo Seiki)

Tear strength: Tear strength is expressed in the value obtained bydividing the force required for the tearing of the film test specimen bythe cross-sectional area of the film test specimen. The unit is N/cm.

Test conditions: Test was conducted in accordance with JIS Z1702. Oneend of the film test specimen was set to the fixed clamp and the otherend of the film was set to the clamp connected to the tester. A notch 20mm long was made in the central part of the 2.5-mm distance between theclamps in the tearing direction by means of the blade of the testequipment, and the pendulum was released to tear the test specimen. Theenergy required to tear the 43-mm section of the remaining uncut portionof the specimen was determined.

(2) Film impact:

The impact strength of plastic film was determined, and the unit isexpressed in KJ/m.

Test equipment: Film impact tester (available from Toyo Seiki)

Test conditions: Film test specimens, 100 mm×100 mm, were used. After atest specimen was set in the equipment by means of air clamps, impactdestruction energy was determined by punching through the specimen withan impact head (head diameter: 1.27 mm).

(3) Stiffness:

The toughness of plastic film was determined, and the unit is expressedin MPa.

Test equipment: Film stiffness tester (available from Toyo Seiki)

Test conditions: A film test specimen was deflected upward in a convexshape by means of a film stiffness tester. The top of the convex-shapedspecimen was pressed, and the load at the time of a specified amount ofdeflection was read to determine the toughness of the specimen.

(4) Average peel strength:

A laminated film consisting of the 4-methyl-1-pentene polymer layer andnylon layer laminated via an adhesive resin layer was delaminated, andthe peel strength was determined to measure the adhesion of the film.

Peel strength: Force required to delaminate a laminated film specimencut out in a dumbbell 15 mm wide. The unit is N/15 mm.

Test equipment: Universal testing machine, Model 2005, available fromIsotesco

Test conditions: A laminated film specimen previously cut out in a shapeof dumbbell 15 mm wide is delaminated partially. Both ends of thepartially delaminated test specimen is mounted on the testing machine inthe T-shaped form and peeled at a rate of 300 mm/min to determine anaverage of the measurements of the peel strength.

Examples 1 to 10, Comparative Examples 1 to 5

Resin compositions having the formulations as shown in Table 2 belowwere prepared under the melting and blending conditions described above.The modification rates of the modified polyolefin resins and the resincompositions obtained therefrom are as shown in Table 2.

Using the resin compositions thus obtained as an intermediate layer,laminates comprising a 4-methyl-pentene-1 polymer/resincomposition/nylon 6 were obtained under the conditions for the formationof extruded multi-layer cast film as described above. The laminates thusobtained were put to peeling test to determine the interlaminaradhesion. The results are shown in Table 2.

Further, the modification rate in Table 2 is the rate (wt %) of thetotal amount of the maleic anhydride in modifying the polymers, (B-1a),(B-1b) and (B-2), against the total resin amount[(A)+(B-1a)+(B-1b)+(B-2)+(C)].

                  TABLE 2                                                         ______________________________________                                                                   Modifi-                                               Formulation of cation Av. Peel                                               Example Adhesive Resin Layer (wt %) rate Strength                           No.    (A)    (B-1a)  (B-1b)                                                                              (B-2)                                                                              (C) (wt %)                                                                              (N/15 mm)                          ______________________________________                                        Ex. 1  84     1       0     15   0   0.18  6.8                                  Ex. 2 82 3 0 15 0 0.29 6.2                                                    Ex. 3 80 5 0 15 0 0.36 15.3                                                   Ex. 4 47.5 5 0 47.5 0 0.625 16.1                                              Comp. 50 0 0 50 0 0.5 2                                                       Ex. 1                                                                         Ex. 5 54 1 0 15 30 0.18 10.1                                                  Ex. 6 52 3 0 15 30 0.24 16.4                                                  Comp. 55 0 0 15 30 0.15 0.13                                                  Ex. 2                                                                         Comp. 55 0 0 30 15 0.3 0.88                                                   Ex. 3                                                                         Ex. 7 50 5 0 15 30 0.425 14                                                   Ex. 8 50 5 0 30 15 0.65 30                                                    Ex. 9 45 5 0 35 15 0.725 20                                                   Ex. 10 50 0 5 30 15 0.35 4.0                                                  Comp. 50 0 0 35 15 0.525 0.34                                                 Ex. 4                                                                         Comp. 80 20 0 0 0 0.6 2.57                                                    Ex. 5                                                                       ______________________________________                                    

The above results indicate that Comparative Example 1 not containing the(B-1) component shows lower adhesion (average peel strength) to nylon 6than Example 4 containing both (B-1) and (B-2) components. Further, inthe case of the systems containing the (C) component, ComparativeExamples 2 to 4 not containing the (B-1) component show lower adhesion(average peel strength) to nylon 6 than Examples 5 to 9 containing both(B-1) and (B-2) components.

Comparative Example 5, not containing the (B-2) component, has loweradhesion than Example 3.

Next, the physical properties of the laminates of the aforementionedExample 6 and Comparative Example 5 were determined by the method asdescribed above. The results are shown in Table 3.

                  TABLE 3                                                         ______________________________________                                                        Example 6                                                                              Comp. Example 5                                      ______________________________________                                        Elmendorf tear strength (N/cm):                                                 MD 205 173                                                                    TD 978 930                                                                    Film impact (KJ/m) 20.1 17.6                                                  Stiffness (MPa)                                                               MD 16.0 18.8                                                                  TD 14.6 9.5                                                                   Average peel strength (N/15 mm) 16.4 2.57                                     Peeled condition after peel test Destruction of Simply peeled                  material of condition                                                         peeled surface                                                             ______________________________________                                    

Table 3 indicates that the laminates of the present invention haveexcellent film impact and tear strength as well.

Examples 11 to 14

The adhesion to EVOH of the laminates using 4-methyl-1-pentene polymercompositions of the present invention used in Examples 2, 4, 5 and 6 asthe adhesive resin was evaluated by the method as described below. Theresults are shown in Table 4 below.

Method for determining the adhesion of the lamination of EVOH/adhesiveresin/4-methyl-1-pentene polymer:

The laminate samples were prepared by overlaying EVOH film, adhesiveresin film and 4-methyl-1-pentene polymer film so that the laminatestructure was as shown below, and press-molded under the conditionsshown below.

Laminate structure: EVOH/adhesive resin/4-methyl-1-pentene polymer=1.0mm/0.1 mm/1.0 mm

Resins used: EVOH

Adhesive resin: A compound obtained by blending the components as shownin Table 1 at the compounding ratios shown in Table 2.

4-methyl-1-pentene polymer: 4-methyl-1-pentene/1-decene copolymer[1-decene content: 6.5 wt %; MFR(temp.:260° C.; load: 5 kg): 20 g/10min, produced by Mitsui Chemicals]

Press-molding conditions:

Pressing temp.: 270° C.

Pressing time: 6 min

Pressing pressure: 6 MPa

                  TABLE 4                                                         ______________________________________                                        Adhesive resin Composition                                                                          Av. Peel Strength (MPa)                                 ______________________________________                                        Example 11                                                                            Composition of Example 2                                                                        9.50                                                  Example 12 Composition of Example 4 9.71                                      Example 13 Composition of Example 5 7.87                                      Example 14 Composition of Example 6 13.12                                   ______________________________________                                    

Further, laminates prepared by using 4-methyl-1-pentene polymer and EVOHalone but without using any composition of the present invention werealso tested under the same conditions, but they did not bond with eachother at all.

From the above it can be seen that the compositions of the presentinvention are also effective for the bonding of 4-methyl-1-pentenepolymer and EVOH.

What we claim is:
 1. A 4-methyl-1-pentene polymer compositioncomprising:(a) 25 to 95 wt % of a 4-methyl-1-pentene polymer (A); and(b) 5 to 75 wt % of a modified polyolefin resin (B) comprising a mixtureof an unsaturated carboxylic acid-modified 4-methyl-1-pentene polymer(B-1) whose polymer is a homopolymer of 4-methyl-1-pentene or of acopolymer containing not less than 85 mol % of the 4-methyl-1-pentenecomponent and an unsaturated carboxylic acid-modified ethylene/α-olefincopolymer (B-2).
 2. A 4-methyl-1-pentene polymer compositioncomprising:(a) 25 to 90 wt % of a 4-methyl-1-pentene polymer (A); (b1)0.1 to 20 wt % of an unsaturated carboxylic acid-modified4-methyl-1-pentene polymer (B-1) whose polymer is a homopolymer of4-methyl-1-pentene or of a copolymer containing not less than 85 mol %of the 4-methyl-1-pentene component; (b2) 4 to 60 wt % of an unsaturatedcarboxylic acid-modified ethylene/α-olefin copolymer (B-2); and (c) 5 to50 wt % of a butene-1 polymer (C).
 3. A 4-methyl-1-pentene polymercomposition as claimed in claim 1, which comprises 25 to 90 wt % of the4-methyl-1-pentene polymer (A), 0.1 to 20 wt % of the unsaturatedcarboxylic acid-modified 4-methyl-1-pentene polymer (B-1), 4 to 60 wt %of the unsaturated carboxylic acid-modified ethylene/α-olefin copolymer(B-2), and 5 to 50 wt % of a butene-1 polymer (C), wherein the totalamount of the unsaturated carboxylic acid-modified 4-methyl-1-pentenepolymer (B-1) and the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) is 5 to 75 wt %.
 4. A4-methyl-1-pentene polymer composition as claimed in claim 3, whereinthe rate of modification of the unsaturated carboxylic acid-modified4-methyl-1-pentene polymer (B-1) is 0.01 to 10 wt %.
 5. A4-methyl-1-pentene polymer composition as claimed in claim 3, whereinthe rate of modification of the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) is 0.01 to 10 wt %.
 6. A4-methyl-1-pentene polymer composition as claimed in claim 3, whereinthe 4-methyl-1-pentene polymer (A) is a homopolymer of4-methyl-1-pentene or a copolymer containing not less than 85 mol % ofthe 4-methyl-1-pentene component.
 7. A 4-methyl-1-pentene polymercomposition as claimed in claim 1, wherein the rate of modification ofthe modified polyolefin resin (B) is 0.01 to 10 wt %.
 8. A4-methyl-1-pentene polymer composition as claimed in claim 1, whereinthe concentration of the unsaturated carboxylic acid-modified4-methyl-1-pentene polymer (B-1) in the composition is 0.1 to 20 wt %and the concentration of the unsaturated carboxylic acid-modifiedethylene/α-olefin copolymer (B-2) in the composition is 4 to 65 wt %. 9.A 4-methyl-1-pentene polymer composition as claimed in 8, 1 or 2,wherein the rate of modification of the unsaturated carboxylicacid-modified 4-methyl-1-pentene polymer (B-1) is 0.01 to 10 wt %.
 10. A4-methyl-1-pentene polymer composition as claimed in claim 1 or 2,wherein the rate of modification of the unsaturated carboxylicacid-modified ethylene/α-olefin copolymer (B-2) is 0.01 to 10 wt %. 11.A 4-methyl-1-pentene polymer composition as claimed in claim 1 or 2,wherein the 4-methyl-1-pentene polymer (A) is a homopolymer of4-methyl-1-pentene or a copolymer containing not less than 85 mol % ofthe 4-methyl-1-pentene component.
 12. An adhesive comprising a4-methyl-1-pentene polymer composition as claimed in claim 1 or
 2. 13.An adhesive as claimed in claim 12, which is used for bonding a4-methyl-1-pentene polymer and a resin containing a polar group.